Qin Wei, Jain Rishabh, Robles Hernández Francisco C, Rimer Jeffrey D
Department of Chemical and Biomolecular Engineering, University of Houston, Houston, TX, 77204, USA.
Department of Mechanical Engineering Technology, University of Houston, Houston, TX, 77204, USA.
Chemistry. 2019 Apr 23;25(23):5893-5898. doi: 10.1002/chem.201901067. Epub 2019 Mar 29.
Zeolite crystals can be used as seeds or aluminosilicate sources in syntheses to control polymorphs and/or reduce the quantity of organics used as structure-directing agents. A frequently invoked hypothesis for interzeolite transformations is that zeolites share some underlying similarity in structure, most notably in cases pertaining to organic-free syntheses. Herein, we show for the first time that ZSM-5 (MFI) can be directly obtained from USY (FAU) through an interzeolite transformation between parent-daughter structures lacking common building units in the absence of a structure-directing agent and seeds. We show that interzeolite transformation leads to a crystalline product with fewer defects. Our findings also reveal that ZSM-5 is a metastable intermediate that undergoes further transformation to mordenite (MOR) and quartz. The MFI-to-MOR transition is counter to reported trends for which transformations lead to structures with reduced molar volume. Herein, we propose mechanistic arguments that suggest the driving force for interzeolite transformation is more complex than guidelines posited in the literature.
沸石晶体可在合成中用作晶种或硅铝酸盐源,以控制多晶型物和/或减少用作结构导向剂的有机物用量。关于沸石间转变,一个经常被提及的假设是,沸石在结构上存在一些潜在的相似性,在无有机合成的情况下尤其如此。在此,我们首次表明,ZSM-5(MFI)可在无结构导向剂和晶种的情况下,通过缺乏共同结构单元的母-子结构间的沸石间转变直接由USY(FAU)制得。我们表明,沸石间转变会产生缺陷较少的晶体产物。我们的研究结果还揭示,ZSM-5是一种亚稳中间体,会进一步转变为丝光沸石(MOR)和石英。从MFI到MOR的转变与报道的转变趋势相反,报道的趋势是转变会导致摩尔体积减小的结构。在此,我们提出了一些机理论据,表明沸石间转变的驱动力比文献中提出的指导原则更为复杂。